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Soviet Journal of Quantum Electronics

Relationship between the threshold pump power and the quenching of stimulated emission from complex molecules

V. V. Gruzinskii, С. В. Давыдов

Published Mar 31, 1976• 0 citations
Publisher

Abstract

A system of rate equations is used to find the conditions under which stimulated emission from organic compounds continues at pump powers W below the threshold Wth. An analysis is made of the dependence of this phenomenon on the temporal characteristics of the active medium and pump radiation, and on the pump power.
DOI
10.1070/qe1976v006n03abeh011082

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An analysis is made of the dynamics of the electronic spectra of complex molecules associated with the nuclear motion, and of its manifestation on exposure of a molecule to high-power optical radiation. A model is proposed for the inhomogeneous broadening dynamics. This describes the random walk of the spectral frequency in the form of a Gauss-Markov random process and allows for the relaxation of the spectra which accompanies an electronic transition. Simple readily interpreted relationships, which describe the influence of nuclear relaxation on the stimulated emission frequency, are obtained.
A calculation is made of the stimulated emission threshold of organic dye solutions as a function of the diffusion coefficient, intensity of induced singlet–singlet or triplet–triplet absorption at the stimulated emission wavelength, steepness of the leading edge of pump pulses, and other parameters. It is shown that, if the dipole moment of a fluorescence transition is perpendicular to the dipole moments of associated induced singlet–singlet or triplet–triplet absorption transitions, the laser threshold of high–viscosity solutions is considerably lower than that of low-viscosity systems. The maximum value of the ratio of the cross sections of the singlet-singlet absorption and stimulated emission, at which a given molecule ceases to emit stimulated radiation, increases from 1 to 3 when the rotational diffusion coefficient decreases from ∞ to 0.
A theoretical study is made of the influence of changes in the relaxation of a three-level system in a resonance field on the dispersion, absorption, and difference between the populations of levels activated by noncoherent pumping. This change in the relaxation is due to a tendency of a thermal reservoir to create an additional difference between the populations of quasienergy states that appear under the influence of the resonance field. It is shown that as a consequence there is a considerable change in the nature of the interaction with the radiation field in laser crystals with three-level active centers when the pump power is close to the threshold. The lasing conditions are found subject to such changes. It is shown that the threshold pump power can be reduced in this case to a value at which the difference between the populations of the active levels vanishes and lasing appears because of an inversion of the populations in a system of quasienergy levels. Under transient conditions the lasing frequency near the threshold should then depend on the pump
The threshold pump power density for lasing in dye solutions is found to depend on the photon energy of pumping radiation. An increase in the pumping photon energy can significantly lower the threshold pump power of dye lasers. For an ethanol solution of rhodamine 6G with a concentration of 4×10 18 cm −3 , the threshold power density for pumping radiation with a wavelength of 532 nm is 20-fold higher than for pumping radiation with a wavelength of 347 nm. This phenomenon is associated with the competition of collective spontaneous emission, which can lead to the efficient deactivation of excited molecules in femtosecond times, and the dephasing of excited molecules due to the intramolecular nonradiative processes of absorbed-energy conversion. An increase in the dephasing rate with the increasing energy of exciting photons lowers the efficiency of collective spontaneous emission and increases the concentration of dephased excited molecules responsible for lasing.
Solutions of the rate equations for a two-level system describing spectral properties in the presence of stimulated emission under picosecond-pulse pumping conditions are examined. The materials of interest are broad band tunable, vibronic laser crystals whose lasing properties under normal pumping conditions have been related to spectral properties through the McCumber theory1. The population inversion at threshold can then be determined by three methods: lifetime shortening, band narrowing, and peak gain measurements.